title: Fifth-order three-dimensional electronic spectroscopy using a pump-probe configuration.
abstract: We present the theoretical details and experimental demonstration of fifth-order three-dimensional (3D) electronic spectroscopy using a pump-probe beam geometry. This is achieved using a pulse shaper and appropriate phase cycling schemes. We show how 8-step and 27-step phase cycling schemes can measure purely absorptive 3D spectra as well as 3D spectra for the individual fifth-order processes that contribute to the purely absorptive spectrum. 3D spectra as a function of two separate controllable waiting time periods can be obtained. The peak shapes and positions of the peaks in the experimental measurement correspond well to theory.
authors.affiliation: Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University , 21 Nanyang Link, Singapore 637371.
authors.forename: Zhengyang
authors.initials: Z
authors.lastname: Zhang
authors.forename: Kym L
authors.initials: KL
authors.lastname: Wells
authors.forename: Marco T
authors.initials: MT
authors.lastname: Seidel
authors.forename: Howe-Siang
authors.initials: HS
authors.lastname: Tan